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Cited by 213Electrocatalysts for Energy ConversionHydrogen Storage and MaterialsCO2 Reduction Techniques and Catalysts

Optimizing Hydrogen Binding on Ru Sites with RuCo Alloy Nanosheets for Efficient Alkaline Hydrogen Evolution

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Cai, Chao, Liu, Kang, Zhu, Yuanmin, Li, Pengcheng, Wang, Qiyou, Liu, Bao, Chen, Shanyong, Li, Huangjingwei +10 more·2022·Angewandte Chemie International Edition
DOI 10.1002/anie.202113664PMC PMC9300137
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Abstract

Ruthenium (Ru)‐based catalysts, with considerable performance and desirable cost, are becoming highly interesting candidates to replace platinum (Pt) in the alkaline hydrogen evolution reaction (HER). The hydrogen binding at Ru sites (Ru−H) is an important factor limiting the HER activity. Herein, density functional theory (DFT) simulations show that the essence of Ru−H binding energy is the strong interaction between the orbital of Ru and the 1s orbital of H. The charge transfer between Ru sites and substrates (Co and Ni) causes the appropriate downward shift of the ‐band center of Ru, which results in a Gibbs free energy of 0.022 eV for H* in the RuCo system, much lower than the 0.133 eV in the pure Ru system. This theoretical prediction has been experimentally confirmed using RuCo alloy‐nanosheets (RuCo ANSs). They were prepared via a fast co‐precipitation method followed with a mild electrochemical reduction. Structure characterizations reveal that the Ru atoms are embedded into the Co substrate as isolated active sites with a planar symmetric and Z‐direction asymmetric coordination structure, obtaining an optimal modulated electronic structure. Hydrogen sensor and temperature program desorption (TPD) tests demonstrate the enhanced Ru−H interactions in RuCo ANSs compared to those in pure Ru nanoparticles. As a result, the RuCo ANSs reach an ultra‐low overpotential of 10 mV at 10 mA cm −2 and a Tafel slope of 20.6 mV dec −1 in 1 M KOH, outperforming that of the commercial Pt/C. This holistic work provides a new insight to promote alkaline HER by optimizing the metal‐H binding energy of active sites.

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  • Traditional supports on the micrometer scale are usually not compatible with catalysts on the nanoscale and therefore do not contribute considerably to the intrinsic catalytic activity.

    “traditional supports on the micrometer scale are usually not compatible with the catalysts on the nanoscale and therefore do not contribute considerably to the intrinsic catalytic activity.”

    From An energy-saving support made of silver nanowire aerogel for hydrogen evolution reaction (2023) · cites this paper as [31]

    Our copy describes how Ru sites embedded in Co nanosheets improve hydrogen binding and catalytic activity (section labeled Abstract; page unavailable). It does not address whether traditional micrometer-scale supports are incompatible with nanoscale catalysts or make little contribution to intrinsic activity. Searches for “micrometer” and “traditional supports” found no passage making that claim. (LLM, conf=0.74)

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Authors
Cai, C., Liu, K., Zhu, Y., Li, P., Wang, Q., Liu, B., Chen, S., Li, H., Zhu, L., Li, H., Fu, J., Chen, Y., Pensa, E., Hu, J., Lu, Y., Chan, T., Cortés, E., & Liu, M.
Affiliations
  • Central South University (CN)
  • Southern University of Science and Technology (CN)
  • Ludwig-Maximilians-Universität München (DE)
  • Zhengzhou University (CN)
  • National Synchrotron Radiation Research Center (TW)
Corresponding author
  • Cortés, Emiliano
  • Liu, Min
ORCID
Venue
Angewandte Chemie International Edition
Publisher
Wiley
Published
2021-12-07
Volume
61
Issue
4
Pages
e202113664-e202113664
ISSN
  • 1433-7851 (ISSN-L)
  • 1521-3773
DOI
10.1002/anie.202113664
PMC
PMC9300137
OpenAlex
W3217607620
Cited by
213
References
60
Citations by year
2026: 32 · 2025: 40 · 2024: 43 · 2023: 54 · 2022: 43 · 2021: 1
FWCI
6.61
Type
journal article
Language
en
Open access
Licence
Locations
  • Angewandte Chemie International Edition (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • Spiral (Imperial College London) (submittedVersion, cc-by)
Funders
European Commission (ERC-STG 802989)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Materials Science › Materials Chemistry › Hydrogen Storage and Materials
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Keywords
alkaline hydrogen evolution reaction, ruthenium catalysts, metal-hydrogen interaction, charge transfer, band center shift, platinum-free electrocatalysts, co-precipitation synthesis, electrochemical reduction, hydrogen adsorption, overpotential

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